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<p>Electroreduction derived Cu-based two-dimensional materials have emerged as promising catalysts for the electroreduction of CO<sub>2</sub> to C<sub>2+</sub> products; however, it remains ambiguous whether the reconstructed interface structures significantly impact the reduction performance. Herein, we first fabricate interface-engineered Cu nanosheets via <i>in situ</i> pre-electrolysis of kilogram-scale brochantite nanosheets precursors, in which lead underpotential deposition reveals the presence of abundant Cu(100)/Cu(110) interfaces, confirmed by OH<sup>−</sup> electrosorption analysis. <i>In situ</i> attenuated total reflection-surface enhanced infrared absorption spectroscopy elucidates the C–C coupling pathways involving the hydrogenation of *CO intermediates to form *CHO species, followed by their subsequent coupling to generate *COCHO. <i>Operando</i> Raman spectra demonstrate that the abundant interfaces provide sufficient *CO surface coverage, thereby facilitating the subsequent deep coupling reactions. Moreover, density-functional-theory calculations indicate the Cu(100)/Cu(110) interfaces reduce the energy barriers of rate-determining hydrogenation step by 0.16 eV and promote the coupling of *CO and *CHO. As a result, the Cu nanosheets with rich Cu(100)/Cu(110) interfaces achieve a remarkable C<sub>2+</sub> Faradaic efficiency of 80.4% at a current density of 800 mA cm<sup>−2</sup>, surpassing most reported Cu-based catalysts.</p>

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In situ reconstructed interface-engineered Cu nanosheets for industrial-current-density CO2 electroreduction to C2+ products

  • 期刊论文

  • 发表日期：

    2025年6月4日

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  • Qiong Wu,
  • Runhua Chen,
  • Juncheng Zhu,
  • Shumin Wang,
  • Yang Wu,
  • Yongfu Sun

摘要

Electroreduction derived Cu-based two-dimensional materials have emerged as promising catalysts for the electroreduction of CO2 to C2+ products; however, it remains ambiguous whether the reconstructed interface structures significantly impact the reduction performance. Herein, we first fabricate interface-engineered Cu nanosheets via in situ pre-electrolysis of kilogram-scale brochantite nanosheets precursors, in which lead underpotential deposition reveals the presence of abundant Cu(100)/Cu(110) interfaces, confirmed by OH− electrosorption analysis. In situ attenuated total reflection-surface enhanced infrared absorption spectroscopy elucidates the C–C coupling pathways involving the hydrogenation of *CO intermediates to form *CHO species, followed by their subsequent coupling to generate *COCHO. Operando Raman spectra demonstrate that the abundant interfaces provide sufficient *CO surface coverage, thereby facilitating the subsequent deep coupling reactions. Moreover, density-functional-theory calculations indicate the Cu(100)/Cu(110) interfaces reduce the energy barriers of rate-determining hydrogenation step by 0.16 eV and promote the coupling of *CO and *CHO. As a result, the Cu nanosheets with rich Cu(100)/Cu(110) interfaces achieve a remarkable C2+ Faradaic efficiency of 80.4% at a current density of 800 mA cm−2, surpassing most reported Cu-based catalysts.